300% Enhancement of Carrier Mobility in Uniaxial-Oriented Perovskite Films Formed by Topotactic-Oriented Attachment

Organic–inorganic perovskites with intriguing optical and electrical properties have attracted significant research interests due to their excellent performance in optoelectronic devices. Recent efforts on preparing uniform and large-grain polycrystalline perovskite films have led to enhanced carrier lifetime up to several microseconds. However, the mobility and trap densities of polycrystalline perovskite films are still significantly behind their single-crystal counterparts. Here, a facile topotactic-oriented attachment (TOA) process to grow highly oriented perovskite films, featuring strong uniaxial-crystallographic texture, micrometer-grain morphology, high crystallinity, low trap density (≈4 × 10¹⁴ cm⁻³), and unprecedented 9 GHz charge-carrier mobility (71 cm² V⁻¹ s⁻¹), is demonstrated. TOA-perovskite-based n-i-p planar solar cells show minimal discrepancies between stabilized efficiency (19.0%) and reverse-scan efficiency (19.7%). The TOA process is also applicable for growing other state-of-the-art perovskite alloys, including triple-cation and mixed-halide perovskites.